络合物的形成对对苯醌的费米共振的影响
摘要
费米共振是一种广泛存在于分子内和分子间的分子振动耦合和能量转移现象。费米共振研究不仅在物理学中的分子振动电子态相互耦合,分子结构与性能等研究中有重要理论意义,而且在材料、生物、化学中的谱线认证、归属、酶分子构型的确定,抗癌药物疗效的考证,地质学中包裹分析,晶体中杂质检测,声学、光学器件研制等都有重要应用。随着光学仪器和量子力学的进步和发展,费米共振研究不断深入,研究结果表明,费米共振蕴藏着丰富的理论和应用潜力。费米共振还有很多规律有待认知,还有很多实际应用问题有待解决。
我们用改变二元溶液浓度的方法研究了CS2在C6H6中费米共振的变化；通过改变联苯分子的压强,分析了压强对联苯分子费米共振的影响；使用液芯光纤技术获得了对苯醌与脯氨酸形成络合物的拉曼光谱并探讨了对苯醌与脯氨酸相互作用生成络合物对对苯醌分子费米共振的影响,取得了以下创新性成果：
(1)二元溶液(CS2在C6H6中)不同浓度对费米共振的影响
发生费米共振的因素除分子内部因素外,还与分子所处的物质形态,环境等有很大的关系。对气态、液态、固态的费米共振等已有很多人员进行了研究。在溶液中,溶质和溶剂分子间发生各种相互作用,会引起分子某些基团的振动频率、散射系数(相对强度)发生变化,这些变化都会引起分子的费米共振现象的改变。频率变化对费米共振影响研究较多,而相对强度变化对费米共振影响的研究还未见过报导。
因此,我们测量了CS：在C6H6中不同浓度的拉曼光谱。并观察到溶液中的ν1-2ν2费米共振明显与纯CS2中不同。用J. F. Berttern方程,计算了费米共振特性参数。结果表明,随着浓度降低,两光谱强度比R减小,耦合系数W增加,其它参数△、△0、K122等也发生相应变化。实验中还观察到ν1和2ν2线并非对称移动,利用G. Fini, D. G. Rea等人的溶剂效应研究结果给予了解释,即此现象是由溶剂效应和CS2在C6H6中的ν1谱线散射系数(相对强度)发生较大变化引起的。研究结果表明,当两振动光谱频率差、光谱强度差都较大时,J.F. Berttern公式应该加以修正。此研究对溶液中谱线认证及理解费米共振微观机理有参考意义。
(2)压力对联苯分子的费米共振的影响
随着有机光电二极管和激光器的迅猛发展,聚苯化合物在光电器件方面的应用备受关注,振动光谱可以给出丰富的分子空间构象信息,对于此类聚合物的费米共振的研究也成为讨论的热点。
因此,我们测量了0-15GPa压强下联苯分子的拉曼光谱。实验结果表明,随压强增加,分子内和分子间π-π共轭和离域效应增强,谱线的绝对强度变大、蓝移。联苯分子的两费米共振谱线强度比R。减少,频率差△增加,当压强为8GPa时,费米共振现象消失,利用J. F. Betran理论得出了固有频率差△0和耦合系数W随压强的变化关系,通过高压下相变进行了解释,并探讨了高压下费米共振耦合变弱的机理。
(3)络合物的产生对对苯醌费米共振的影响
费米共振是简单分子中普遍存在的现象如：CO2、CS2中的费米共振已有大量研究文章。那么在复杂的大分子、络合物、聚合物中更是存在着很多费米共振现象。我们在研究过程中发现在络合物、聚合物研究中一些谱线难以归属的原因之一就是往往没有考虑到费米共振现象。在络合物中由于分子间的相互作用,使某些基团振动频率、偶极矩、极化率发生变化,或者由于配位等作用使基团对称性发生变化。这些因素会使参与络合的分子原有的费米共振发生变化,也可能产生新的费米共振。
本文对对苯醌与氨基酸相互作用生成n-π*电荷转移络合物的费米共振进行了研究。对苯醌与氨基酸相互作用研究一直是备受关注的热门课题。关于两种分子相互作用生成什么产物也是多年一直争论的话题。本文的研究证明了：不同的pH值产生不同的产物,在强碱性(pH=11)的条件下生成电荷转移络合物。在已进行的光谱法研究中所获得的络合物拉曼光谱强度都比较弱小。本研究使用Teflon液芯光纤共振拉曼技术,大幅度的提高了拉曼光谱强度,获得了高质量的10-4 M浓度的对苯醌与脯氨酸生成的络合物的拉曼光谱,将其与对苯醌的拉曼光谱相比较发现有很大的变化,其变化的机理是络合物形成过程中脯氨酸的N原子上的自由电子转移到对苯醌的π反键轨道上,处于激发态脱离刀轨道的电子云使对苯醌的C=O、C=C、C-C苯环等基团振动频率、极化率等发生不同程度的变化,与其相关的费米共振也发生了变化。本文对形成络合物后的对苯醌的C=O、C-C键的费米共振进行了分析,并与文献中的结果进行了比较。结果是C=0键的费米共振发生很大变化而C-C键的费米共振变化很小。这一定性分析结果对络合物的光谱研究中的谱线的归属、认证给出了一种思路和线索。
Fermi resonance is a widely present in the intramolecular and inter-molecular vibration coupling and energy transfer phenomena. The research of Fermi resonance, has theoretical significance in the coupling between electronic states of molecular vibration and molecular structure research of Physics. And it also has been widely used in subjects such as Material science, Biology, Chemistry. Medical, Geology, Acoustics and Optics. By the development of optical instruments and Quantum Mechanics, Fermi resonance studies have advanced by scientists, and the results have proved this research has great potential. There are still many questions waiting about Fermi resonance to be confirmed.
We had studied the Fermi resonance in the solution of two constituents with the method of change the concentration of the solution, and the solution contain CS2 and C6H6; by changing the pressure of biphenyl molecule, we analyzed the effect of pressure on the biphenyl molecule's Fermi resonance; we also used liquid-core optical fiber to get the Raman spectra of proline-benzoquinone complex, studied the effect of the complex on the p-Benzoquinone's Fermi resonance, and achieved the following results of innovative:
(1) Effect of different concentration binary solution (CS2 inside of C6H6) to Fermi resonance
Except for molecular internal factors of Fermi resonance, its also has a great relationship to physical form, the environment of molecular. Gaseous, liquid, solid-state Fermi resonance has been studied by a lot of staff. In solution, various interactions in solute and solvent molecules will cause certain groups molecular vibration frequencies and scattering coefficient (relative intensity) changes, all this changes will cause changes of molecular Fermi resonance. The study for impact of frequency change to Fermi resonance has been done by lots of people, but the study for effect of relative intensity to the Fermi resonance have not yet seen the report.
Therefore, we measured the Raman spectra of C6H6 and CS2 in different concentrations and observed the Fermi resonance which is obviously different with pure CS2.We calculated the characteristic parameters with the equation of J.F.Berttern. The results state clearly that the ratio of the two spectral intensity decreases, the coupling coefficient increases and other parameters also change by the reduction of concentration. We also observed that the line v1and 2v2are not moving symmetrically which is explained by G.F ini and D.G.R effects. That is. this phenomenon is caused by solvent effects and great changes have taken place in the spectrum line scattering coefficient (relative strength). The results of the study show that the J.F.Berttern formula should be revised when two vibration spectral frequencies and spectral intensity have big difference. The study has significant reference meaning on solution spectral lines and understanding the Fermi resonance authentication microscopic mechanism.
(2) Effects of pressure on biphenyl's Fermi resonance
As organic photodiode and laser device developing rapidly, the use of polyphenylene compound in photoelectric devices has caused great attention. Since vibration spectrum contains conformational information of molecular space. research on Polymer's Fermi resonance has become hot issue.
In this experiment. Raman spectrum of biphenyl molecule has been measured under the pressure of 0-15GPa. Result shows that as pressure increase, the intramolecular and intermolecularπ-πconjugation and delocalization effect enhanced and the absolute intensity of spectral line increased and blue shifted. The ratio (R(?)) of intensity of biphenyl molecule's Fermi resonance line decreased and the frequency difference increased. When pressure reached 8GPa. Fermi resonance disappeared. The relationship between natural frequency differenceΔ0 and coupling constant w under different pressure can be calculated with J. F. Betran's Theory and interpreted by high pressure phase transition approach. In the paper also discussed Fermi resonance coupling's weakening mechanism under high pressure.
(3) The effects of formation of complexOn the Fermi resonance of p-benzoquinone
Fermi Resonance is the phenomenon commonly found in simple molecules, and it has so many papers for the fermi Resonance researching of CO2, CS2. So accordingly there is more Fermi Resonances in complex molecules, complexes, polymers. In the course of the study, we find that some Spectrums in the complex, polymer are difficult to confirm the source, which is largely due to losing sight of the Fermi Resonance phenomenon. In the complex, the interaction between molecules would change some groups vibration frequency, dipole moment and polarization ratios. Simultaneously the Groups symmetry-may be transformed by the role of coordination too. All these factors would make a difference of the previous Fermi Resonance in the involved complex molecules.or produce new Fermi resonance.
This paper studied the complex's Fermi resonance, the n-πcharge transfer complex is produced by the interaction between p-benzoquinone and amino acids. The interaction between p-Benzoquinone and amino acid has been hot topics of concerning in the physics. Similarly, the topic for the products of Interaction between the two molecules has been arguing for years. In the work, the present result confirm:different pH values produce different products, and it would creat new complex with electric charge transferring in the condition of Alkaline (pH=11). In the spectrometry research, we obtained complex Raman intensities are relatively weaker. Our research used Teflon resonance Raman spectra in liquid-core optical fiber technology, enhanced the Laman spectral intensity greatly, and gained high quality Raman spectra of the 10-4M proline-benzoquinone complex. There are great changes when comparing this spectra with the Raman spectra of p-benzoquinone. The reason is. during the complex formation proline's free electron which was belong to the N atom transfered to theπanti-bonding orbital of p-benzoquinone, the electron cloud in excited state that had left the orbit changed vibration frequency and polarization of p-benzoquinone's C=O,C=C,C-C bond, the related Fermi resonance is also changed.
This article has analyze the Fermi resonance of benzoquinone C=O. C-C bond after forming complex, and also compare to the result of document. The result is that C=O bond Fermi resonance change enormous but C-C bond Fermi resonance changes little. idea and clue have been given by this result about spectral line attribution and certification in complex spectroscopy.
我们用改变二元溶液浓度的方法研究了CS2在C6H6中费米共振的变化；通过改变联苯分子的压强,分析了压强对联苯分子费米共振的影响；使用液芯光纤技术获得了对苯醌与脯氨酸形成络合物的拉曼光谱并探讨了对苯醌与脯氨酸相互作用生成络合物对对苯醌分子费米共振的影响,取得了以下创新性成果：
(1)二元溶液(CS2在C6H6中)不同浓度对费米共振的影响
发生费米共振的因素除分子内部因素外,还与分子所处的物质形态,环境等有很大的关系。对气态、液态、固态的费米共振等已有很多人员进行了研究。在溶液中,溶质和溶剂分子间发生各种相互作用,会引起分子某些基团的振动频率、散射系数(相对强度)发生变化,这些变化都会引起分子的费米共振现象的改变。频率变化对费米共振影响研究较多,而相对强度变化对费米共振影响的研究还未见过报导。
因此,我们测量了CS：在C6H6中不同浓度的拉曼光谱。并观察到溶液中的ν1-2ν2费米共振明显与纯CS2中不同。用J. F. Berttern方程,计算了费米共振特性参数。结果表明,随着浓度降低,两光谱强度比R减小,耦合系数W增加,其它参数△、△0、K122等也发生相应变化。实验中还观察到ν1和2ν2线并非对称移动,利用G. Fini, D. G. Rea等人的溶剂效应研究结果给予了解释,即此现象是由溶剂效应和CS2在C6H6中的ν1谱线散射系数(相对强度)发生较大变化引起的。研究结果表明,当两振动光谱频率差、光谱强度差都较大时,J.F. Berttern公式应该加以修正。此研究对溶液中谱线认证及理解费米共振微观机理有参考意义。
(2)压力对联苯分子的费米共振的影响
随着有机光电二极管和激光器的迅猛发展,聚苯化合物在光电器件方面的应用备受关注,振动光谱可以给出丰富的分子空间构象信息,对于此类聚合物的费米共振的研究也成为讨论的热点。
因此,我们测量了0-15GPa压强下联苯分子的拉曼光谱。实验结果表明,随压强增加,分子内和分子间π-π共轭和离域效应增强,谱线的绝对强度变大、蓝移。联苯分子的两费米共振谱线强度比R。减少,频率差△增加,当压强为8GPa时,费米共振现象消失,利用J. F. Betran理论得出了固有频率差△0和耦合系数W随压强的变化关系,通过高压下相变进行了解释,并探讨了高压下费米共振耦合变弱的机理。
(3)络合物的产生对对苯醌费米共振的影响
费米共振是简单分子中普遍存在的现象如：CO2、CS2中的费米共振已有大量研究文章。那么在复杂的大分子、络合物、聚合物中更是存在着很多费米共振现象。我们在研究过程中发现在络合物、聚合物研究中一些谱线难以归属的原因之一就是往往没有考虑到费米共振现象。在络合物中由于分子间的相互作用,使某些基团振动频率、偶极矩、极化率发生变化,或者由于配位等作用使基团对称性发生变化。这些因素会使参与络合的分子原有的费米共振发生变化,也可能产生新的费米共振。
本文对对苯醌与氨基酸相互作用生成n-π*电荷转移络合物的费米共振进行了研究。对苯醌与氨基酸相互作用研究一直是备受关注的热门课题。关于两种分子相互作用生成什么产物也是多年一直争论的话题。本文的研究证明了：不同的pH值产生不同的产物,在强碱性(pH=11)的条件下生成电荷转移络合物。在已进行的光谱法研究中所获得的络合物拉曼光谱强度都比较弱小。本研究使用Teflon液芯光纤共振拉曼技术,大幅度的提高了拉曼光谱强度,获得了高质量的10-4 M浓度的对苯醌与脯氨酸生成的络合物的拉曼光谱,将其与对苯醌的拉曼光谱相比较发现有很大的变化,其变化的机理是络合物形成过程中脯氨酸的N原子上的自由电子转移到对苯醌的π反键轨道上,处于激发态脱离刀轨道的电子云使对苯醌的C=O、C=C、C-C苯环等基团振动频率、极化率等发生不同程度的变化,与其相关的费米共振也发生了变化。本文对形成络合物后的对苯醌的C=O、C-C键的费米共振进行了分析,并与文献中的结果进行了比较。结果是C=0键的费米共振发生很大变化而C-C键的费米共振变化很小。这一定性分析结果对络合物的光谱研究中的谱线的归属、认证给出了一种思路和线索。
Fermi resonance is a widely present in the intramolecular and inter-molecular vibration coupling and energy transfer phenomena. The research of Fermi resonance, has theoretical significance in the coupling between electronic states of molecular vibration and molecular structure research of Physics. And it also has been widely used in subjects such as Material science, Biology, Chemistry. Medical, Geology, Acoustics and Optics. By the development of optical instruments and Quantum Mechanics, Fermi resonance studies have advanced by scientists, and the results have proved this research has great potential. There are still many questions waiting about Fermi resonance to be confirmed.
We had studied the Fermi resonance in the solution of two constituents with the method of change the concentration of the solution, and the solution contain CS2 and C6H6; by changing the pressure of biphenyl molecule, we analyzed the effect of pressure on the biphenyl molecule's Fermi resonance; we also used liquid-core optical fiber to get the Raman spectra of proline-benzoquinone complex, studied the effect of the complex on the p-Benzoquinone's Fermi resonance, and achieved the following results of innovative:
(1) Effect of different concentration binary solution (CS2 inside of C6H6) to Fermi resonance
Except for molecular internal factors of Fermi resonance, its also has a great relationship to physical form, the environment of molecular. Gaseous, liquid, solid-state Fermi resonance has been studied by a lot of staff. In solution, various interactions in solute and solvent molecules will cause certain groups molecular vibration frequencies and scattering coefficient (relative intensity) changes, all this changes will cause changes of molecular Fermi resonance. The study for impact of frequency change to Fermi resonance has been done by lots of people, but the study for effect of relative intensity to the Fermi resonance have not yet seen the report.
Therefore, we measured the Raman spectra of C6H6 and CS2 in different concentrations and observed the Fermi resonance which is obviously different with pure CS2.We calculated the characteristic parameters with the equation of J.F.Berttern. The results state clearly that the ratio of the two spectral intensity decreases, the coupling coefficient increases and other parameters also change by the reduction of concentration. We also observed that the line v1and 2v2are not moving symmetrically which is explained by G.F ini and D.G.R effects. That is. this phenomenon is caused by solvent effects and great changes have taken place in the spectrum line scattering coefficient (relative strength). The results of the study show that the J.F.Berttern formula should be revised when two vibration spectral frequencies and spectral intensity have big difference. The study has significant reference meaning on solution spectral lines and understanding the Fermi resonance authentication microscopic mechanism.
(2) Effects of pressure on biphenyl's Fermi resonance
As organic photodiode and laser device developing rapidly, the use of polyphenylene compound in photoelectric devices has caused great attention. Since vibration spectrum contains conformational information of molecular space. research on Polymer's Fermi resonance has become hot issue.
In this experiment. Raman spectrum of biphenyl molecule has been measured under the pressure of 0-15GPa. Result shows that as pressure increase, the intramolecular and intermolecularπ-πconjugation and delocalization effect enhanced and the absolute intensity of spectral line increased and blue shifted. The ratio (R(?)) of intensity of biphenyl molecule's Fermi resonance line decreased and the frequency difference increased. When pressure reached 8GPa. Fermi resonance disappeared. The relationship between natural frequency differenceΔ0 and coupling constant w under different pressure can be calculated with J. F. Betran's Theory and interpreted by high pressure phase transition approach. In the paper also discussed Fermi resonance coupling's weakening mechanism under high pressure.
(3) The effects of formation of complexOn the Fermi resonance of p-benzoquinone
Fermi Resonance is the phenomenon commonly found in simple molecules, and it has so many papers for the fermi Resonance researching of CO2, CS2. So accordingly there is more Fermi Resonances in complex molecules, complexes, polymers. In the course of the study, we find that some Spectrums in the complex, polymer are difficult to confirm the source, which is largely due to losing sight of the Fermi Resonance phenomenon. In the complex, the interaction between molecules would change some groups vibration frequency, dipole moment and polarization ratios. Simultaneously the Groups symmetry-may be transformed by the role of coordination too. All these factors would make a difference of the previous Fermi Resonance in the involved complex molecules.or produce new Fermi resonance.
This paper studied the complex's Fermi resonance, the n-πcharge transfer complex is produced by the interaction between p-benzoquinone and amino acids. The interaction between p-Benzoquinone and amino acid has been hot topics of concerning in the physics. Similarly, the topic for the products of Interaction between the two molecules has been arguing for years. In the work, the present result confirm:different pH values produce different products, and it would creat new complex with electric charge transferring in the condition of Alkaline (pH=11). In the spectrometry research, we obtained complex Raman intensities are relatively weaker. Our research used Teflon resonance Raman spectra in liquid-core optical fiber technology, enhanced the Laman spectral intensity greatly, and gained high quality Raman spectra of the 10-4M proline-benzoquinone complex. There are great changes when comparing this spectra with the Raman spectra of p-benzoquinone. The reason is. during the complex formation proline's free electron which was belong to the N atom transfered to theπanti-bonding orbital of p-benzoquinone, the electron cloud in excited state that had left the orbit changed vibration frequency and polarization of p-benzoquinone's C=O,C=C,C-C bond, the related Fermi resonance is also changed.
This article has analyze the Fermi resonance of benzoquinone C=O. C-C bond after forming complex, and also compare to the result of document. The result is that C=O bond Fermi resonance change enormous but C-C bond Fermi resonance changes little. idea and clue have been given by this result about spectral line attribution and certification in complex spectroscopy.
引文
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